The aim of this work is to examine the adsorption performance and mechanism of phosphorus (P) onto polyethyene polyamine (PEPA) grafted chitosan-zirconium(IV) composite beads (CS-Zr-PEPA) from aqueous solutions. The morphology, functional groups, and surface area of the CS-Zr-PEPA beads were characterized by SEM, FTIR, and BET analysis. Batch adsorption experiments were conducted via different operating parameters such as solution pH, initial phosphate concentration, co-existing anions and temperature. The adsorption kinetics, equilibrium isotherms and adsorption stability of the adsorbent were scrutinized. In comparison with other CS-based beads, the CS-Zr-PEPA had a greater affinity towards P and exhibited a maximum adsorption capacity of 103.96 mg-P/g predicted by Langmuir mode. The reusability studies of CS-Zr-PEPA beads were carried out. The CS-Zr-PEPA beads exhibit preferable sequestration of P through specific interactions, as further demonstrated by studying physicochemical characteristics of the virgin beads and P-adsorbed beads using X-ray photoelectron spectroscopy (XPS). The column performance of CS-Zr-PEPA beads was tested with P-containing wastewater. Results indicated that the developed CS-Zr-PEPA composite beads could be utilized as a promising adsorbent for effective removal and recovery of P from water and wastewater.